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Artificial iron hydrogenase made by covalent grafting of Knolker's complex into xylanase: Application in asymmetric hydrogenation of an aryl ketone in water

Kariyawasam, Kalani, Ghattas, Wadih, de los Santos, Yossef Lopez, Doucet, Nicolas ORCID: https://orcid.org/0000-0002-1952-9380, Gaillard, Sylvain, Renaud, Jean-Luc, Avenier, Frederic, Mahy, Jean-Pierre et Ricoux, Rémy (2020). Artificial iron hydrogenase made by covalent grafting of Knolker's complex into xylanase: Application in asymmetric hydrogenation of an aryl ketone in water Biotechnology and Applied Biochemistry , vol. 67 , nº 4. p. 563-573. DOI: 10.1002/bab.1906.

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Résumé

We report a new artificial hydrogenase made by covalent anchoring of the iron Knolker's complex to a xylanase S212C variant. This artificial metalloenzyme was found to be able to catalyze efficiently the transfer hydrogenation of the benchmark substrate trifluoroacetophenone by sodium formate in water, yielding the corresponding secondary alcohol as a racemic. The reaction proceeded more than 3-fold faster with the XlnS212CK biohybrid than with the Knolker's complex alone. In addition, efficient conversion of trifluoroacetophenone to its corresponding alcohol was reached within 60 h with XlnS212CK, whereas a approximately 2.5 fold lower conversion was observed with Knolker's complex alone as catalyst. Moreover, the data were rationalized with a computational strategy suggesting the key factors of the selectivity. These results suggested that the Knolker's complex was most likely flexible and could experience free rotational reorientation within the active-site pocket of Xln A, allowing it to access the subsite pocket populated by trifluoroacetophenone.

Type de document: Article
Mots-clés libres: Knölker's complex; artificial metalloenzymes; catalysis; hydrogenation
Centre: Centre INRS-Institut Armand Frappier
Date de dépôt: 15 juill. 2021 00:56
Dernière modification: 15 févr. 2022 15:36
URI: https://espace.inrs.ca/id/eprint/11527

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